Recently, multiferroics-defined as materials with coexistence of at least two of the ferroelectric, ferroelastic and ferromagnetic effects-have attracted enormous research activities. In this thesis, the structure and properties of multiferrioic BiFeO3-x%PbTiO3 and Fe-x%Ga crystalline solutions were investigated.

First, the results show that modified BiFeO3-PbTiO3 based ceramics have significantly enhanced multiferroic properties, relative to BiFeO3 single crystals. The data reveal: (i) a dramatic increase in the induced polarization; and (ii) the establishment of a remnant magnetization by a breaking of the translational invariance of a long-period cycloidal spin structure, via substituent effects. In addition, temperature dependent magnetic permeability investigations of BiFeO3-xPbTiO3 crystalline solutions have shown that aliovalent La substitution results in a significant increase in the permeability.

Second, room temperature high-resolution neutron and x-ray diffraction studies have been performed on Fe-x%Ga crystals for 12